Kinetic energy operator approach to the quantum three-body problem with Coulomb interactions

We present a non-variational, kinetic energy operator approach to the solution of quantum three-body problem with Coulomb interactions, based on the utilization of symmetries intrinsic to the kinetic energy operator, i.e., the three-body Laplacian operator with the respective masses. Through a four-step reduction process, the nine dimensional problem is reduced to a one dimensional coupled system of ordinary differential equations, amenable to accurate numerical solution as an infinite-dimensional algebraic eigenvalue problem. A key observation in this reduction process is that in the functional subspace of the kinetic energy operator where all the rotational degrees of freedom have been projected out, there is an intrinsic symmetry which can be made explicit through the introduction of Jacobi-spherical coordinates. A numerical scheme is presented whereby the Coulomb matrix elements are calculated to a high degree of accuracy with minimal effort, and the truncation of the linear equations is carried out through a systematic procedureComment: 56 pages, 11 figure

The genesis of the quantum theory of the chemical bond

An historical overview is given of the relevant steps that allowed the genesis of the quantum theory of the chemical bond, starting from the appearance of the new quantum mechanics and following later developments till approximately 1931. General ideas and some important details are discussed concerning molecular spectroscopy, as well as quantum computations for simple molecular systems performed within perturbative and variational approaches, for which the Born-Oppenheimer method provided a quantitative theory accounting for rotational, vibrational and electronic states. The novel concepts introduced by the Heitler-London theory, complemented by those underlying the method of the molecular orbitals, are critically analyzed along with some of their relevant applications. Further improvements in the understanding of the nature of the chemical bond are also considered, including the ideas of one-electron and three-electron bonds introduced by Pauling, as well as the generalizations of the Heitler-London theory firstly performed by Majorana, which allowed the presence of ionic structures into homopolar compounds and provided the theoretical proof of the stability of the helium molecular ion. The study of intermolecular interactions, as developed by London, is finally examined.Comment: amsart, 34 pages, 2 figure

Spin and rotational symmetries in unrestricted Hartree Fock states of quantum dots

Ground state energies are obtained using the unrestricted Hartree Fock method for up to four interacting electrons parabolically confined in a quantum dot subject to a magnetic field. Restoring spin and rotational symmetries we recover Hund first rule. With increasing magnetic field, crossovers between ground states with different quantum numbers are found for fixed electron number that are not reproduced by the unrestricted Hartree Fock approximation. These are consistent with the ones obtained with more refined techniques. We confirm the presence of a spin blockade due to a spin mismatch in the ground states of three and four electrons.Comment: 16 Pages, 2 figures, accepted for publication on New Journal of Physic

Floating Wigner molecules and possible phase transitions in quantum dots

A floating Wigner crystal differs from the standard one by a spatial averaging over positions of the Wigner-crystal lattice. It has the same internal structure as the fixed crystal, but contrary to it, takes into account rotational and/or translational symmetry of the underlying jellium background. We study properties of a floating Wigner molecule in few-electron spin-polarized quantum dots, and show that the floating solid has the lower energy than the standard Wigner crystal with fixed lattice points. We also argue that internal rotational symmetry of individual dots can be broken in arrays of quantum dots, due to degenerate ground states and inter-dot Coulomb coupling.Comment: 6 pages incl 3 figure